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Solution coating of large-area organic semiconductor thin films with aligned single-crystalline domains


Solution coating of organic semiconductors offers great potential for achieving low-cost manufacturing of large-area and flexible electronics. However, the rapid coating speed needed for industrial-scale production poses challenges to the control of thin-film morphology. Here, we report an approach—termed fluid-enhanced crystal engineering (FLUENCE)—that allows for a high degree of morphological control of solution-printed thin films. We designed a micropillar-patterned printing blade to induce recirculation in the ink for enhancing crystal growth, and engineered the curvature of the ink meniscus to control crystal nucleation. Using FLUENCE, we demonstrate the fast coating and patterning of millimetre-wide, centimetre-long, highly aligned single-crystalline organic semiconductor thin films. In particular, we fabricated thin films of 6,13-bis(triisopropylsilylethynyl) pentacene having non-equilibrium single-crystalline domains and an unprecedented average and maximum mobilities of 8.1±1.2 cm2 V−1 s−1 and 11 cm2 V−1 s−1. FLUENCE of organic semiconductors with non-equilibrium single-crystalline domains may find use in the fabrication of high-performance, large-area printed electronics.

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Figure 1: Fluid-flow-enhanced crystal growth.
Figure 2: Solution-sheared single-crystalline TIPS-pentacene thin film.
Figure 3: Domain alignment and crystal quality of the single-crystalline TIPS-pentacene films versus that of reference samples.
Figure 4: Grazing-incidence X-ray diffraction images of TIPS-pentacene films for varying solution concentration.
Figure 5: Comparison of transistor characteristics between single-crystalline domain (blue) and reference samples (red) of non-equilibrium TIPS-pentacene.


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This work is supported by the Department of Energy, Laboratory Directed Research and Development funding, under contract DE-AC02-76SF00515 (Y.D.). We are grateful to M. Toney at Stanford Synchrotron Radiation Lighsource (SSRL) for valuable input. We give thanks to J. E. Anthony and M. M. Nelson of 3M for providing high-purity TIPS-pentacene. We appreciate helpful discussions with O. Goto from the Chemical Engineering department at Stanford. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the US DOE, Office of Basic Energy Sciences. B.C-K.T. acknowledges support from a National Science Scholarship from the Agency for Science, Technology and Research (A*STAR), Singapore. G.G., H.A.B. and Z.B. acknowledge support from the National Science Foundation DMR-Solid State Chemistry (DMR-0705687-002). J.X. and G.X. acknowledge the National Science Foundation of China (NSFC 51133002) for financial support. D.H.K. and Z.B. acknowledge the support by the Center for Advanced Molecular Photovoltaics, award no. KUS-C1-015-21, made by King Abdullah University of Science and Technology. R.M.S. acknowledges financial support from the National Science Foundation Graduate Research Fellowship Program. T.H.L. acknowledges support from Toshiba through the Stanford CIS-FMA programme and the ILJU foundation in South Korea.

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Authors and Affiliations



Z.B., S.C.B.M. and Y.D. conceived and designed the experiments. B.C-K.T. fabricated micropillar-patterned shearing blades, and performed photolithography and scanning electron microscopy. Y.D. and J.X. performed solution coating. Y.D. carried out numerical simulation, performed morphology characterizations and conducted device testing. Y.D., G.G. and S.C.B.M. performed X-ray diffraction measurements and data analysis. D.H.K. and T.H.L. advised on surface functionalization and device testing. H.A.B. and R.M.S. contributed to the initial design of the structured shearing blade. Y.D. wrote the first draft of the manuscript. All authors discussed the results and revised the manuscript. Z.B. and S.C.B.M. directed the project.

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Correspondence to Stefan C. B. Mannsfeld or Zhenan Bao.

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Diao, Y., Tee, BK., Giri, G. et al. Solution coating of large-area organic semiconductor thin films with aligned single-crystalline domains. Nature Mater 12, 665–671 (2013).

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